期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 55, 期 31, 页码 8873-8877出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201600463
关键词
heterogeneous catalysis; oxidative dehydrogenation; scanning probe microscopy; surface chemistry; surface structures
资金
- United States Department of Energy (DOE) through the University of California at Davis [DE-FG02-03ER46057]
- Laboratory Directed Research and Development (LDRD) Program: Chemical Imaging Initiative at Pacific Northwest National Laboratory (PNNL)
- Environmental Molecular Sciences Laboratory (EMSL)
- DOE's Office of Biological and Environmental Research
- DOE [DE-AC05-76RL01830]
Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) has been used to image the basal {001} plane of the catalytically relevant M1 phase in MoVTeNb complex oxides. Facets {010}, {120}, and {210} are identified as the most frequent lateral termination planes of the crystals. Combination of STEM with He ion microscopy (HIM) images, Rietveld analysis, and kinetic tests reveals that the activation of ethane is correlated to the availability of facets {001}, {120}, and {210} at the surface of M1 crystals. The lateral facets {120} and {210} expose crystalline positions related to the typical active centers described for propane oxidation. Conversely, the low activity of the facet {010} is attributed to its configuration, consisting of only stable M6O21 units connected by a single octahedron. Thus, we quantitatively demonstrated that differences in catalytic activity among M1 samples of equal chemical composition depend primarily on the morphology of the particles, which determines the predominant terminating facets.
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